Journal
JOURNAL OF CHEMICAL PHYSICS
Volume 130, Issue 24, Pages -Publisher
AIP Publishing
DOI: 10.1063/1.3155081
Keywords
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Funding
- Naval Research Laboratory
- Office of Naval Research
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Decomposition of energetic molecules such as pentaerythritol tetranitrate is accompanied by extensive changes in their electronic configuration and thus is challenging for ab initio Born-Oppenheimer molecular dynamics simulations. The performance of single-determinant methods (in particular, density-functional theory) is validated on electronic structure and molecular dynamics simulations of RO-NO2 bond dissociation in a smaller nitric ester, ethyl nitrate. Accurate description of dissociating molecule requires using unrestricted, spin-symmetry-broken orbitals. However, the iterative self-consistent field procedure is prone to convergence failures in the bond-breaking region even if robust convergence algorithms are employed. As a result, molecular dynamics simulations of unimolecular decomposition need to be closely monitored and manually restarted to ensure seamless transition from the closed-shell to open-shell configuration. (C) 2009 American Institute of Physics. [DOI: 10.1063/1.3155081]
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